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1.
Article in English | MEDLINE | ID: mdl-27960653

ABSTRACT

The aim of this study was to quantify the interactions between graphene oxide (GO) and quartz sand by conducting experimental and modeling analyses. The results show that both GO and quartz sand were negatively charged in the presence of 0-50 mM NaCl and 5 mM CaCl2 (GO = -43.10 to -17.60 mV, quartz sand = -40.97 to -8.44 mV). In the Derjaguin-Landau-Verwey-Overbeek (DLVO) energy profiles, the adhesion of GO to quartz sand becomes more favorable with increasing NaCl concentration from 0 to 10 mM because the interaction energy profile was compressed and the primary maximum energy barrier was lowered. At 50 mM NaCl and 5 mM CaCl2, the primary maximum energy barrier even disappeared, resulting in highly favorable conditions for GO retention to quartz sand. In the Maxwell model analysis, the probability of GO adhesion to quartz sand (αm) increased from 2.46 × 10-4 to 9.98 × 10-1 at ionic strengths of 0-10 mM NaCl. In the column experiments (column length = 10 cm, inner diameter = 2.5 cm, flow rate = 0.5 mL min-1), the mass removal (Mr) of GO in quartz sand increased from 5.4% to 97.8% as the NaCl concentration was increased from 0 to 50 mM, indicating that the mobility of GO was high in low ionic strength solutions and decreased with increasing ionic strength. The Mr value of GO at 5 mM CaCl2 was 100%, demonstrating that Ca2+ had a much stronger effect than Na+ on the mobility of GO. In addition, the mobility of GO was lower than that of chloride (Mr = 1.4%) but far higher than that of multi-walled carbon nanotubes (Mr = 87.0%) in deionized water. In aluminum oxide-coated sand, the Mr value of GO was 98.1% at 0 mM NaCl, revealing that the mobility of GO was reduced in the presence of metal oxides. The transport model analysis indicates that the value of the dimensionless attachment rate coefficient (Da) increased from 0.11 to 4.47 as the NaCl concentration was increased from 0 to 50 mM. In the colloid filtration model analysis, the probability of GO sticking to quartz sand (αf) increased from 6.23 × 10-3 to 2.52 × 10-1 as the NaCl concentration was increased from 0 to 50 mM.


Subject(s)
Graphite/chemistry , Oxides/chemistry , Quartz/chemistry , Water Pollutants, Chemical/chemistry , Models, Theoretical
2.
Article in English | MEDLINE | ID: mdl-28920769

ABSTRACT

The aim of this study was to investigate Cr(VI) removal from chromium-plating rinse water using modacrylic anion-exchange fibers (KaracaronTM KC31). Batch experiments were performed with synthetic Cr(VI) solutions to characterize the KC31 fibers in Cr(VI) removal. Cr(VI) removal by the fibers was affected by solution pH; the Cr(VI) removal capacity was the highest at pH 2 and decreased gradually with a pH increase from 2 to 12. In regeneration and reuse experiments, the Cr(VI) removal capacity remained above 37.0 mg g-1 over five adsorption-desorption cycles, demonstrating that the fibers could be successfully regenerated with NaCl solution and reused. The maximum Cr(VI) removal capacity was determined to be 250.3 mg g-1 from the Langmuir model. In Fourier-transform infrared spectra, a Cr = O peak newly appeared at 897 cm-1 after Cr(VI) removal, whereas a Cr-O peak was detected at 772 cm-1 due to the association of Cr(VI) ions with ion-exchange sites. X-ray photoelectron spectroscopy analyses demonstrated that Cr(VI) was partially reduced to Cr(III) after the ion exchange on the surfaces of the fibers. Batch experiments with chromium-plating rinse water (Cr(VI) concentration = 1178.8 mg L-1) showed that the fibers had a Cr(VI) removal capacity of 28.1-186.4 mg g-1 under the given conditions (fiber dose = 1-10 g L-1). Column experiments (column length = 10 cm, inner diameter = 2.5 cm) were conducted to examine Cr(VI) removal from chromium-plating rinse water by the fibers under flow-through column conditions. The Cr(VI) removal capacities for the fibers at flow rates of 0.5 and 1.0 mL min-1 were 214.8 and 171.5 mg g-1, respectively. This study demonstrates that KC31 fibers are effective in the removal of Cr(VI) ions from chromium-plating rinse water.


Subject(s)
Acrylic Resins/chemistry , Anion Exchange Resins/chemistry , Chromium/analysis , Polyvinyl Chloride/chemistry , Wastewater/chemistry , Water Pollutants, Chemical/analysis , Water Purification/methods , Adsorption , Chromium/chemistry , Hydrogen-Ion Concentration , Water Pollutants, Chemical/chemistry
3.
Water Environ Res ; 88(11): 2111-2120, 2016 Nov 01.
Article in English | MEDLINE | ID: mdl-28661327

ABSTRACT

The aim of this study was to investigate the Cr(VI) adsorption to magnetic iron oxide(MIO) nanoparticle- multi-walled carbon nanotubes (MWCNTs) in aqueous solutions using batch experiments. Results show that the maximum adsorption capacity of Cr(VI) to MIO-MWCNTs was 11.256 mg/g. Kinetic model analysis demonstrates that the pseudo-second-order model and Elovich model are suitable for describing the kinetic data. Thermodynamic analysis indicates that Cr(VI) adsorption to MIO-MWCNTs decreased with increasing temperature from 5-60 °C, indicating the spontaneous and exothermic nature of the sorption process. Equilibrium isotherm analysis demonstrates that the Redlich-Peterson model suitably describes the equilibrium data. In the pH experiments, Cr(VI) adsorption to MIO-MWCNTs decreased gradually from 5.70-2.13 mg/g with increasing pH from 3.0-7.3. Sequential extraction indicates that, among the five binding forms of Cr(VI) associated with MIO-MWCNTs, the predominant contributions are the fraction bound to Fe-Mn oxides (57.82%) and the residual (23.38%).


Subject(s)
Chromium/chemistry , Ferric Compounds/chemistry , Magnetics , Nanoparticles/chemistry , Nanotubes, Carbon/chemistry , Adsorption , Apraxia, Ideomotor , Models, Theoretical , Thermodynamics , Water Pollutants, Chemical/chemistry
4.
Water Environ Res ; 86(12): 2338-46, 2014 Dec.
Article in English | MEDLINE | ID: mdl-25654937

ABSTRACT

Mesoporous iron oxide, particularly amine-functionalized FeO(x) and FeO(x), was investigated for the removal of toxic heavy metal anions of arsenic and chromium from an aqueous solution. As a control experiment for these toxic compounds, adsorption tests were also performed on Fe3O4 as their counterpart bulk chemical. The mesostructures were confirmed by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) and transmission electron microscopy (TEM). In addition, we prepared stock suspensions of meso-FeO(x), amine-functionalized meso-FeO(x) and Fe3O4 particles, and compared their acute toxicity against Daphnia magna. The 24 h-EC50 values of the amine-functionalized meso-FeO(x), meso-FeO(x) and Fe particle suspensions used in this study were 1682, 2549 and 95 mg/L, respectively. Organism toxicity caused by spills of adsorbents can be negated when the amine-functionalized meso-FeO(x), up to 1500 mg/L, is used as the adsorbent for heavy metal treatment. The adsorption of arsenic and chromium by the three adsorbents were examined, and different adsorption models were used to describe the equilibrium and kinetic data. The amine-functionalized meso-FeO(x) adsorbent was found to give the maximum adsorption capacities for arsenic and chromium (33.51 and 25.05 mg/g, respectively). This research gives promising results for the application of modified meso-FeO(x) as an adsorbent of toxic heavy metal anions from aqueous solutions.


Subject(s)
Ferric Compounds/chemistry , Ferric Compounds/toxicity , Magnetite Nanoparticles/chemistry , Magnetite Nanoparticles/toxicity , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/toxicity , Adsorption , Animals , Anions/chemistry , Arsenic/chemistry , Chromium/chemistry , Chromium/toxicity , Daphnia/drug effects , Kinetics , Lethal Dose 50 , Microscopy, Electron, Transmission , Models, Theoretical , Porosity , X-Ray Diffraction
5.
Article in English | MEDLINE | ID: mdl-24844892

ABSTRACT

The aim of this study was to investigate the adsorption of bacteriophage MS2 by magnetic iron oxide nanoparticles in aqueous solutions. The characteristics of synthetic nanoparticles were analyzed using various techniques. The adsorption of MS2 to the nanoparticles was examined under various conditions using batch experiments. The results showed that the nanoparticles were mainly composed of maghemite along with goethite. The nanoparticles had a specific surface area of 82.2 m(2) g(-1), with an average pore diameter of 13.2 nm and total pore volume of 0.2703 cm(3) g(-1). The results demonstrated that the removal of MS2 by the nanoparticles was very fast. A 3.15 log removal (99.93%) was achieved within 60 min (adsorbent dose = 2 g L(-1); MS2 concentration = 2.94 × 10(6) pfu mL(-1)). The log removal decreased from 3.52 to 0.36 with increasing MS2 concentration from 1.59 × 10(4) to 5.01 × 10(7) pfu mL(-1). Also, the effect of solution pH on MS2 removal was minimal at pH 4.2-8.4. The removal of MS2 decreased in the presence of anions such as carbonate and phosphate, with the latter showing a greater hindrance effect on removal. This study demonstrated that magnetic iron oxide nanoparticles are very effective in the removal of MS2 from aqueous solutions.


Subject(s)
Ferric Compounds/chemistry , Iron Compounds/chemistry , Levivirus/chemistry , Metal Nanoparticles/chemistry , Minerals/chemistry , Water Pollutants/chemistry , Water Purification/methods , Adsorption , Magnetic Phenomena , Solutions
6.
Environ Technol ; 35(9-12): 1199-207, 2014.
Article in English | MEDLINE | ID: mdl-24701916

ABSTRACT

The aim of this study was to investigate the removal of bacteriophages MS2 and PhiX174 in soils amended with converter furnace steel slag. Column experiments were performed to examine the bacteriophage removal in slag-amended (slag content: 0%, 25%, and 50%) loam soils. For comparison, column experiments were also conducted with Escherichia coli. In addition, chloride (Cl) was used as a conservative tracer to determine transport characteristics. Results showed mass recoveries of Cl of 98.6 +/- 3.5%, indicating that the experiments were conducted successfully. The mass recovery of MS2 was 86.7% in no slag (100% soil), decreasing to 0% in slag contents of 25% and 50%. The mass recovery of PhiX174 decreased from 87.8% to 51.5% with increasing slag content from 0% to 50%. In the case of E. coli, the mass recoveries decreased from 47.0% to 10.5% with increasing slag content from 0% to 50%. In the transport models analyses, the HYDRUS-1D code was used to quantify the sorption parameters from breakthrough curves. For the 100% soil column, a one-site kinetic sorption model was fitted to the data, whereas a two-site kinetic sorption model was fitted for slag-amended (25% and 50% slag) soil data. Results demonstrate that the addition of steel slag to soil enhances the removal of bacteriophages due to the presence of FeO in the steel slag. However, CaO could not contribute to the bacteriophage removal in our experimental conditions because the effluent pH (7.7-8.9) in slag-amended (25% and 50% slag) soils was not high enough to promote the bacteriophage inactivation.


Subject(s)
Bacteriophage phi X 174/isolation & purification , Levivirus/isolation & purification , Oxides/pharmacology , Soil Microbiology , Soil Pollutants/isolation & purification , Bacteriophage phi X 174/drug effects , Levivirus/drug effects , Models, Theoretical
7.
Int J Biol Macromol ; 279(Pt 1): 135161, 2024 Aug 28.
Article in English | MEDLINE | ID: mdl-39214200

ABSTRACT

Diclofenac (DCF) is frequently detected in aquatic environments, emphasizing the critical need for its efficient removal globally. Here, we present the synthesis of Fe(III)-doped ß-CD-grafted chitosan (Fe/ß-CD@CS) cryogel beads designed for adsorbing DCF in aqueous solutions. The beads exhibited an average size of 2.94 ± 0.66 mm and a point of zero charge of 8.03. Adsorption experiments demonstrated that the Langmuir kinetic model provided the most accurate description of the kinetic data, while the Redlich-Peterson isotherm offered the best fit for the equilibrium data. The beads showcased a theoretical maximum adsorption capacity of 712.3 mg/g for DCF, with the adsorption process being identified as exothermic. DCF adsorption on the beads was attributed to hydrogen bonding, metal cation-π interactions, and electrostatic interactions. Reusability tests exhibited that the beads could be regenerated using 0.1 M NaOH. To perform deep learning modeling, adsorption experiments (n = 17), designed utilizing central composite design (CCD), were conducted in duplicate. The CCD framework incorporated input variables such as initial DCF concentration, adsorbent dosage, and solution pH, while the output variable was the DCF removal rate. Utilizing the adsorption data, an artificial neural network (ANN) model was constructed with a topology of 3: 7:10:1, featuring 3 input variables, 7 neurons in the first hidden layer, 10 neurons in the second layer, and 1 output variable. Employing the ANN model data, 3-D response surface plots were generated to elucidate the relationship between input variables and DCF removal rate. Additional adsorption tests were conducted to evaluate the developed ANN model, affirming its reliable predictability for the DCF removal rate. Analysis of the relative importance of the input variables revealed the following order of importance: solution pH (100 %) > adsorbent dosage (75.2 %) > initial DCF concentration (57.7 %).

8.
Chemosphere ; 366: 143404, 2024 Sep 24.
Article in English | MEDLINE | ID: mdl-39326708

ABSTRACT

The increasing presence of pharmaceuticals and personal care products (PPCPs) in aquatic systems pose significant environmental concerns. This study addresses this issue by synthesizing quaternized mesoporous SBA-15 (QSBA) with varied alkyl chain lengths of C1QSBA, C8QSBA, and C18QSBA. QSBA utilizes dual mechanisms: hydrophobic interactions via the alkyl chain and electrostatic attraction/ion exchange via the ammonium group. Diclofenac (DCF) and acetaminophen (ACT) were selected as target PPCPs due to their contrasting dissociation properties and hydrophobicity, which are the main characteristics of PPCPs. The adsorption of DCF and ACT revealed that longer alkyl chains enhanced the adsorption capacity of ACT through hydrophobic interactions, whereas dissociated DCF (DCF-) adsorption was superior owing to its high hydrophobicity (log Kow = 4.5) and electrostatic attraction. pH levels between 6 and 8 resulted in a high affinity for DCF-. Notably, among the three alkyl chains, only C18QSBA exhibited the most effective adsorption for DCF-. These PPCPs adsorption trends were confirmed through molecular simulations of adsorption under conditions in which competing ions coexisted. The molecular simulations show that while DCF- has lower adsorption energy than Cl-, OH-, and H3O+ ions in QSBA, enhancing its adsorption under various pH conditions. Conversely, ACT exhibits a higher adsorption energy, which reduces its adsorption efficiency. This suggests the potential application of QSBA with long alkyl chains in the treatment of highly hydrophobic and negatively charged PPCPs. Furthermore, this study emphasizes the importance of simulating adsorption under competing ion conditions.

9.
Sci Total Environ ; 926: 171753, 2024 May 20.
Article in English | MEDLINE | ID: mdl-38522552

ABSTRACT

Removing perfluoro(2-methyl-3-oxahexanoic) acid (HFPO-DA) in water treatment is hindered by its hydrophobicity and negative charge. Two adsorbents, quaternary-ammonium-functionalized silica gel (Qgel), specifically designed for anionic hydrophobic compounds, and conventional granular activated carbon (GAC) were investigated for HFPO-DA removal. ANOVA results (p â‰ª 0.001) revealed significant effects on initial concentration, contact time, and adsorbent type. Langmuir model-derived capacities were 285.019 and 144.461 mg/g for Qgel and GAC, respectively, with Qgel exhibiting higher capacity irrespective of pH. In column experiments, selective removal of HFPO-DA removal with Qgel was observed; specifically, in the presence of NaCl, the breakthrough time was extended by 10 h from 26 to 36 h. Meanwhile, the addition of NaCl decreased the breakthrough time from 32 to 14 h for GAC. However, in the presence of carbamazepine, neither of the adsorbents significantly changed the breakthrough time for HFPO-DA. Molecular simulations were also used to compare the adsorption energies and determine the preferential interactions of HFPO-DA and salts or other chemicals with Qgel and GAC. Molecular simulations compared adsorption energies, revealing preferential interactions with Qgel and GAC. Notably, HFPO-DA adsorption energy on GAC surpassed other ions during coexistence. Specifically, with Cl- concentrations from 1 to 10 times, Qgel showed lower adsorption energy for HFPO-DA (-62.50 ± 5.44 eV) than Cl- (-52.89 ± 2.59 eV), a significant difference (p = 0.036). Conversely, GAC exhibited comparable or higher adsorption energy for HFPO-DA (-18.33 ± 40.38 eV) than Cl- (-32.36 ± 29.89 eV), with no significant difference (p = 0.175). This suggests heightened selectivity of Qgel for HFPO-DA removal compared to GAC. Consequently, our study positions Qgel as a promising alternative for effective HFPO-DA removal, contributing uniquely to the field. Additionally, our exploration of molecular simulations in predicting micropollutant removal adds novelty to our study.

10.
Environ Technol ; 34(17-20): 2749-56, 2013.
Article in English | MEDLINE | ID: mdl-24527638

ABSTRACT

The objective of this study was to investigate phosphate removal using magnetic alginate-layered double hydroxide (LDH) composites. The magnetic composites were prepared by entrapping synthetic magnetic iron oxide and calcined Mg-Al LDH in polymer matrix (alginate). Results showed that the magnetic composites (2% magnetic iron oxide and 6% calcined Mg-Al LDH) were effective in the removal of phosphate with the sorption capacity of 5.0 +/- 0.1 mgP/g under given experimental conditions (adsorbent dose = 0.05 g in 30 ml solution; initial phosphate concentration = 10 mgP/l; reaction time = 24 h). Both magnetic iron oxide and calcined Mg-Al LDH have the ability to adsorb phosphate, with the latter having much higher sorption capacity. In the magnetic composites, calcined Mg-Al LDH functions as a phosphate adsorbent while magnetic iron oxide provides both magnetic and sorption properties. Results also demonstrated that phosphate sorption to the magnetic composites reached equilibrium at 24 h. The maximum phosphate sorption capacity was determined to be 39.1 mgP/g. In addition, phosphate removal was not sensitive to initial solution pH between 4.1 and 10.2. Only 9% of the phosphate sorption capacity was reduced as the solution pH increased from 4.1 to 10.2. This study demonstrated that magnetic alginate-LDH composites could be used for phosphate removal in combination with magnetic separation.


Subject(s)
Alginates/chemistry , Aluminum Hydroxide/chemistry , Ferric Compounds/chemistry , Magnesium Hydroxide/chemistry , Magnets/chemistry , Phosphates/isolation & purification , Water Purification/methods , Adsorption , Glucuronic Acid/chemistry , Hexuronic Acids/chemistry , Water/analysis
11.
Environ Technol ; 34(5-8): 703-10, 2013.
Article in English | MEDLINE | ID: mdl-23837321

ABSTRACT

The aim of this study was to investigate the adhesion of bacteria (Escherichia coli) to pyrophyllite clay using batch and flow-through column experiments. Batch results demonstrated that pyrophyllite was effective in removing bacteria (94.5 +/- 2.0%) from aqueous solution (1 mM NaCl solution; pyrophyllite dose of 1 g/ml). At solution pH 7.1, negatively-charged bacteria could be removed due to their adhesion to positively-charged surfaces of pyrophyllite (point of zero charge = 9.2). Column results showed that pyrophyllite (per cent removal of 94.1 +/- 2.3%) was far more effective in bacterial adhesion than quartz sand (53.6 +/- 5.3%) under the given experimental conditions (flow rate of 0.3 ml/min; solution of 1 mM NaCl + 0.1 mM NaHCO3). Bacterial removal in pyrophyllite columns increased from 90 to 100% with decreasing flow rate from 0.6 to 0.15 ml/min due to increasing contact time between bacteria and filter materials. In addition, bacterial removal remained relatively constant at 94-97% even though NaHCO3 concentration increased from 0.1 to 10 mM (flow rate of 0.3 ml/min). This could be related to the fact that pyrophyllite remained positively-charged even though the solution conditions changed. This study demonstrates that pyrophyllite could be used as adsorptive filter materials in the removal of bacteria.


Subject(s)
Aluminum Silicates/chemistry , Bacterial Adhesion/physiology , Escherichia coli/isolation & purification , Escherichia coli/physiology , Ultrafiltration/methods , Water Microbiology , Water/chemistry , Adsorption , Clay , Water Purification/methods
12.
Environ Technol ; 34(17-20): 2757-64, 2013.
Article in English | MEDLINE | ID: mdl-24527639

ABSTRACT

In this study, the deposition and transport of Pseudomonas aeruginosa on sandy porous materials have been investigated under static and dynamic flow conditions. For the static experiments, both equilibrium and kinetic batch tests were performed at a 1:3 and 3:1 soil:solution ratio. The batch data were analysed to quantify the deposition parameters under static conditions. Column tests were performed for dynamic flow experiments with KCl solution and bacteria suspended in (1) deionized water, (2) mineral salt medium (MSM) and (3) surfactant + MSM. The equilibrium distribution coefficient (K(d)) was larger at a 1:3 (2.43 mL g(-1)) than that at a 3:1 (0.28 mL g(-1)) soil:solution ratio. Kinetic batch experiments showed that the reversible deposition rate coefficient (k(att)) and the release rate coefficient (k(det)) at a soil:solution ratio of 3:1 were larger than those at a 1:3 ratio. Column experiments showed that an increase in ionic strength resulted in a decrease in peak concentration of bacteria, mass recovery and tailing of the bacterial breakthrough curve (BTC) and that the presence of surfactant enhanced the movement of bacteria through quartz sand, giving increased mass recovery and tailing. Deposition parameters under dynamic condition were determined by fitting BTCs to four different transport models, (1) kinetic reversible, (2) two-site, (3) kinetic irreversible and (4) kinetic reversible and irreversible models. Among these models, Model 4 was more suitable than the others since it includes the irreversible sorption term directly related to the mass loss of bacteria observed in the column experiment. Applicability of the parameters obtained from the batch experiments to simulate the column breakthrough data is evaluated.


Subject(s)
Pseudomonas aeruginosa/cytology , Soil Microbiology , Bacterial Adhesion , Kinetics , Models, Biological , Porosity , Potassium Chloride/chemistry , Silicon Dioxide/chemistry , Surface-Active Agents/chemistry , Water/chemistry
13.
Environ Sci Pollut Res Int ; 30(17): 49703-49719, 2023 Apr.
Article in English | MEDLINE | ID: mdl-36780080

ABSTRACT

Acetaminophen (AAP) is an analgesic and non-steroidal anti-inflammatory drug and a micropollutant that has been detected in waterbodies worldwide. Here, we explore the characteristics of AAP adsorption onto spherical carbons (SCs) hydrothermally synthesized from pure sucrose as a carbon source. In one-factor-at-a-time experiments, the adsorption capacity of AAP remained relatively constant between pH 2 and 10 but became negligible at pH 12. The Raman, FTIR, and XPS spectra illustrate that hydrogen bonding, π-π interactions, and n-π* interactions could contribute to the AAP adsorption onto the SCs. CHEM3D modeling was used to explore hydrogen-bond formation, π-π interactions, n-π* interactions, and electrostatic repulsion between AAP and the SCs. In view of the pHpzc of the SCs (3.1) and the pKa of AAP (10.96), electrostatic repulsion could occur between negatively charged SCs and anionic AAP above pH 10. In consideration of the average pore diameter of the SCs (1.89 nm) and the AAP molecular size (8.94 Å × 7.95 Å × 4.93 Å), a pore-filling mechanism could contribute to the adsorption. A pseudo-second-order model was best fitted to the kinetic data (equilibrium time = 6 h), whereas the Liu isotherm was most suitable for the equilibrium data (maximum adsorption capacity = 92.0 mg/g). Adsorption of AAP to the SCs was exothermic at 10-40 °C. The SCs were regenerated and reused for AAP adsorption using a methanol. Multiple-factor-at-once (MFAO) experiments (input variables: pH, temperature, adsorbent dosage, and initial AAP concentration; output: AAP adsorption capacity) were used to develop response surface methodology (RSM, quartic regression) and artificial neural network (ANN, topology 4:11:9:1) models. Analyses using additional MFAO experimental data reveal that the predictive ability of the ANN model (R2 = 0.890) was better than that of the RSM model (R2 = 0.764). Based on the weight values of the ANN model, the relative importance of the input variables on the output was quantified in the order of initial AAP concentration (100%) > adsorbent dosage (92.3%) > temperature (77.6%) > pH (43.6%).


Subject(s)
Acetaminophen , Water Pollutants, Chemical , Adsorption , Carbon , Temperature , Models, Theoretical , Kinetics , Water Pollutants, Chemical/analysis , Hydrogen-Ion Concentration , Thermodynamics
14.
Chemosphere ; 311(Pt 1): 137074, 2023 Jan.
Article in English | MEDLINE | ID: mdl-36332741

ABSTRACT

Ibuprofen (IPF) is one of the most prescribed nonsteroidal anti-inflammatory drugs in recent times, but it is not readily removed in conventional wastewater treatments. Here, we investigate the adsorption characteristics of IPF onto calcined spherical hydrochar (CSH), which was synthesized through hydrothermal carbonization of sucrose followed by calcination. The adsorption experiments show that the equilibration time for IPF was 360 min, and a pseudo-second-order model was best fitted to the kinetic data. The isotherm data were best described by the Liu model with a theoretical maximum adsorption capacity of 95.6 mg/g. The thermodynamic data indicate the endothermic nature of the adsorption at 10-40 °C. The CSH was favorably regenerated and reused using methanol. In pH experiments, the IPF adsorption capacity declined gradually as pH rose from 2 to 8, dropped rapidly at pH 10, and became negligible at pH 12. The IPF adsorption to the CSH could occur through various adsorption mechanisms. Hydrogen-bond formation, π-π interactions, n-π* interactions, and electrostatic repulsion were explored and visualized with molecular modeling using CHEM3D. The Raman, FTIR, and XPS spectra suggest that π-π interactions could take place between the CSH and IPF. Considering the pKa value of IPF (4.91) and pHiep of the CSH (3.21), electrostatic repulsion between the negatively-charged CSH and anionic IPF could play a negative role in the adsorption. A pore-filling mechanism could contribute to the adsorption in view of the molecular size of IPF (9.43 Å × 7.75 Å × 6.23 Å) and the average pore diameter of the CSH (2.27 nm). In addition, hydrophobic interactions could be involved in the adsorption. Multi-factor adsorption experiments were executed with pH, temperature, CSH dosage, and initial IPF concentrations as input variables and IPF removal rate as an output variable, and an artificial neural network (ANN) model with a topology of 4:9:11:1 was developed to sufficiently describe the adsorption data (R > 0.99). Further analyses with additional experimental data confirm that the ANN model possessed good predictability for multi-factor adsorption.


Subject(s)
Ibuprofen , Water Pollutants, Chemical , Adsorption , Water Pollutants, Chemical/chemistry , Hydrogen-Ion Concentration , Neural Networks, Computer , Kinetics , Thermodynamics
15.
Sci Rep ; 13(1): 5170, 2023 Mar 30.
Article in English | MEDLINE | ID: mdl-36997526

ABSTRACT

Santa Barbara Amorphous-15 (SBA) is a stable and mesoporous silica material. Quaternized SBA-15 with alkyl chains (QSBA) exhibits electrostatic attraction for anionic molecules via the N+ moiety of the ammonium group, whereas its alkyl chain length determines its hydrophobic interactions. In this study, QSBA with different alkyl chain lengths were synthesized using the trimethyl, dimethyloctyl, and dimethyoctadecyl groups (C1QSBA, C8QSBA, and C18QSBA, respectively). Carbamazepine (CBZ) is a widely prescribed pharmaceutical compound, but is difficult to remove using conventional water treatments. The CBZ adsorption characteristics of QSBA were examined to determine its adsorption mechanism by changing the alkyl chain length and solution conditions (pH and ionic strength). A longer alkyl chain resulted in slower adsorption (up to 120 min), while the amount of CBZ adsorbed was higher for longer alkyl chains per unit mass of QSBA at equilibrium. The maximum adsorption capacities of C1QSBA, C8QSBA, and C18QSBA, were 3.14, 6.56, and 24.5 mg/g, respectively, as obtained using the Langmuir model. For the tested initial CBZ concentrations (2-100 mg/L), the adsorption capacity increased with increasing alkyl chain length. Because CBZ does not dissociate readily (pKa = 13.9), stable hydrophobic adsorption was observed despite the changes in pH (0.41-0.92, 1.70-2.24, and 7.56-9.10 mg/g for C1QSBA, C8QSBA, and C18QSBA, respectively); the exception was pH 2. Increasing the ionic strength from 0.1 to 100 mM enhanced the adsorption capacity of C18QSBA from 9.27 ± 0.42 to 14.94 ± 0.17 mg/g because the hydrophobic interactions were increased while the electrostatic attraction of the N+ was reduced. Thus, the ionic strength was a stronger control factor determining hydrophobic adsorption of CBZ than the solution pH. Based on the changes in hydrophobicity, which depends on the alkyl chain length, it was possible to enhance CBZ adsorption and investigate the adsorption mechanism in detail. Thus, this study aids the development of adsorbents suitable for pharmaceuticals with controlling molecular structure of QSBA and solution conditions.

16.
Int J Biol Macromol ; 241: 124516, 2023 Jun 30.
Article in English | MEDLINE | ID: mdl-37086762

ABSTRACT

Mercury (Hg) is widely used in many industrial processes and is released into the environment. Therefore, efficient removal of Hg from water is of vital importance worldwide. Here, we explored the adsorption characteristics of Hg(II) on polyethyleneimine-functionalized carboxymethylcellulose (PEI-CMC) beads and studied the toxicity of the beads toward Daphnia magna and Pseudokirchneriella subcapitata. The PEI-CMC beads had an average particle size of 2.04 ± 0.25 mm, a point of zero charge (pHpzc) of 5.8, and a swelling ratio of 2.45. Acute toxicity tests demonstrated that the PEI-CMC beads had no toxic effects on D. magna. The growth inhibition tests revealed that growth inhibition of P. subcapitata could be attributed to adsorption of trace elements in growth media on the PEI-CMC beads. The adsorption experiments exhibited that the Matthews and Weber model best described the kinetic data, whereas the Redlich-Peterson model was well fitted to the isotherm data. The theoretical maximum Hg(II) adsorption capacity of the PEI-CMC beads was 313.1 mg/g. The thermodynamic experiments showed endothermic nature of the Hg(II) adsorption on the PEI-CMC beads at 10-40 °C. The adsorption experiments exhibited that the Hg(II) adsorption capacity decreased gradually as pH increased from 2 to 12. The adsorption of Hg(II) on the PEI-CMC beads can occur through chelation and electrostatic attraction. The FTIR and XPS spectra before and after Hg(II) adsorption confirmed that chelation of neutral Hg(II) species (HgCl2, HgClOH, and Hg(OH)2) can occur with amino and oxygen-containing functional groups on the PEI-CMC beads. Considering species distribution of Hg(II) and the pHpzc of the PEI-CMC beads, electrostatic attraction between the positively-charged beads and anionic Hg(II) species (HgCl3- and HgCl42-) can take place in highly acidic solutions. The PEI-CMC beads were regenerated and reused for Hg(II) adsorption using 0.1 M HCl.


Subject(s)
Polyethyleneimine , Water Pollutants, Chemical , Polyethyleneimine/chemistry , Carboxymethylcellulose Sodium/chemistry , Adsorption , Kinetics , Toxicity Tests , Water Pollutants, Chemical/toxicity , Water Pollutants, Chemical/chemistry , Hydrogen-Ion Concentration
17.
Water Sci Technol ; 66(4): 761-7, 2012.
Article in English | MEDLINE | ID: mdl-22766864

ABSTRACT

The objective of this study was to investigate the removal of bacteriophages in Mg/Al layered double hydroxide (LDH). Batch experiments were performed with bacteriophage MS2 in a powder form of Mg/Al LDH under various LDH doses. Column experiments were also performed under flow-through condition with bacteriophages MS2 and phiX174 in Mg/Al LDH immobilized on sand surfaces. Batch tests demonstrated that the powder form of Mg/Al LDH was effective in removing MS2 with the removal capacity of 2.2 × 10(8) plaque forming unit (pfu)/g under the given experimental conditions (LDH dose = 2 g/L; initial MS2 concentration = 4.61 × 10(5) pfu/mL). Column experiments showed that the log removal of phiX174 was 4.40 in columns containing 100% Mg/Al LDH-coated sand while it was 0.05 in 100% quartz sand. These findings indicated that Mg/Al LDH-coated sand was effective in removing bacteriophages compared with sand. A more than 4 log removal (=5.44) of MS2 was achieved in 100% Mg/Al LDH-coated sand. This study demonstrates the potential application of Mg/Al LDH for virus removal in water treatment.


Subject(s)
Aluminum Hydroxide , Bacteriophage phi X 174/isolation & purification , Levivirus/isolation & purification , Magnesium Hydroxide , Water Pollutants/isolation & purification , Water Purification/methods , Drug Combinations , Quartz
18.
Article in English | MEDLINE | ID: mdl-22871003

ABSTRACT

The objective of this study was to investigate the removal of the bacteriophage MS2 by Ni/Al layered double hydroxide (LDH). Batch experiments were performed using a powder form of Ni/Al LDH under various conditions. Column experiments were also performed under flow-through conditions with Ni/Al LDH coated sand. Batch tests showed that the powder form of Ni/Al LDH was effective for bacteriophage removal under the given experimental conditions (LDH dose of 2.5 g L(-1); initial MS2 concentration of 1.35 × 10(5) plaque forming unit (pfu) mL(-1)) with a removal capacity of 5.5 × 10(7) pfu g(-1). The results also indicated that the effect of the solution pH on the bacteriophage removal was minimal at pH 4.3-9.4. The influence of divalent anions (SO(2-) (4), CO(2-) (3), HPO(2-) (4); concentrations 1-100 mM) on the removal of the bacteriophage was significant, while the effects of monovalent anions (NO(-) (3), Cl(-)) were negligible. Column experiments showed that the log removal of MS2 was 4.51 in columns containing 100% Ni/Al LDH-coated sand, while it was 0.02 in columns containing 100% quartz sand (initial MS2 concentration of approximately 7.0 × 10(5) pfu mL(-1); flow rate of 0.5 mL min(-1)). These findings indicated that Ni/Al LDH-coated sand was far more effective at removing bacteriophage than sand alone. This study demonstrates that Ni/Al LDH can be used for virus removal in water treatment and filtration applications.


Subject(s)
Aluminum Hydroxide/chemistry , Bacteriophages/isolation & purification , Magnesium Hydroxide/chemistry , Anions/chemistry , Filtration/methods , Water Purification/methods
19.
Article in English | MEDLINE | ID: mdl-22571524

ABSTRACT

The objective of this study was to investigate the performance of iron-manganese bimetallic oxide-coated sand (IMCS) in the removal of bacteria (Escherichia coli ATCC 11105) using small-scale (length = 20 cm, inner diameter = 2.5 cm) and 30-day long-term (length = 50 cm, inner diameter = 2.5 cm) column experiments. Results indicated that the bacterial removal capacity of IMCS (q(eq) = 0.66 g/g) was slightly lower than that of iron oxide-coated sand (ICS) (q(eq) = 0.69 g/g) but about two times greater than those of manganese oxide-coated sand (MCS, q(eq) = 0.30 g/g) and dual media containing ICS and MCS (q(eq) = 0.35 g/g). In IMCS, increasing the flow rate from 0.5 to 3.0 mL/min decreased the removal capacity from 1.14 to 0.64 g/g. Nitrate showed an enhancement effect on the removal capacity of IMCS at 1 and 10 mM, while phosphate and bicarbonate had both hindrance (1 mM) and enhancement (10 mM) effects, depending on their concentrations. The long-term column experiment (bacterial injection conc. = 4.2 × 10(6) CFU/mL) showed that IMCS could remove more than 99.9 % of bacteria within 13 days (effluent conc. = 1.6 × 10(2) CFU/mL). This study demonstrated that IMCS could be used as an adsorptive filter medium for bacterial removal in water treatment.


Subject(s)
Escherichia coli/isolation & purification , Ferric Compounds/metabolism , Filtration/methods , Manganese Compounds/metabolism , Oxides/metabolism , Silicon Dioxide/metabolism , Water Microbiology , Water Purification/methods , Bicarbonates , Escherichia coli/metabolism , Ferric Compounds/chemistry , Manganese Compounds/chemistry , Nitrates , Oxides/chemistry , Phosphates , Silicon Dioxide/chemistry
20.
J Environ Sci (China) ; 24(4): 589-95, 2012.
Article in English | MEDLINE | ID: mdl-22894091

ABSTRACT

The removal of As(III) and As(V) from aqueous solution was investigated using waste cast iron, which is a byproduct of the iron casting process in foundries. Two types of waste cast iron were used in the experiment: grind precipitate dust (GPD) and cast iron shot (CIS). The X-ray diffraction analysis indicated the presence of Feo on GPD and CIS. Batch experiments were performed under different concentrations of As(III) and As(V) and at various initial pH levels. Results showed that waste cast iron was effective in the removal of arsenic. The adsorption isotherm study indicated that the Langmuir isotherm was better than the Freundlich isotherm at describing the experimental result. In the adsorption of both As(IH) and As(V), the adsorption capacity of GPD was greater than CIS, mainly due to the fact that GPD had higher surface area and weight percent of Fe than CIS. Results also indicated the removal of As(III) and As(V) by GPD and CIS was influenced by the initial solution pH, generally decreasing with increasing pH from 3.0 to 10.5. In addition, both GPD and CIS were more effective at the removal of As(III) than As(V) under given experimental conditions. This study demonstrates that waste cast iron has potential as a reactive material to treat wastewater and groundwater containing arsenic.


Subject(s)
Arsenates/isolation & purification , Arsenites/isolation & purification , Iron/chemistry , Waste Products/analysis , Water Pollutants, Chemical/isolation & purification , Adsorption , Chemical Precipitation , Electron Probe Microanalysis , Hydrogen-Ion Concentration , Kinetics , Solutions , Temperature , X-Ray Diffraction
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